Understanding the Adsorption of Rare-Earth Elements in Oligo-Grafted Mesoporous Carbon

Gismondi, Pasquale; Kuzmin, Alexei; Unsworth, Colin; Rangan, Sylvie; Khalid, Syed; Saha, Dipendu

doi:10.1021/acs.langmuir.1c02403

Title: Understanding the Adsorption of Rare-Earth Elements in Oligo-Grafted Mesoporous Carbon

Journal Article · 27 December 2021 · Langmuir

DOI: https://doi.org/10.1021/acs.langmuir.1c02403 · OSTI ID:1842800

Gismondi, Pasquale ^[1];

^[2]; Unsworth, Colin ^[1];

^[3]; Khalid, Syed ^[4];

^[1]

Widener Univ., Chester, PA (United States)
Univ. of Latvia, Riga (Latvia). Inst. of Solid State Physics
Rutgers Univ., Piscataway, NJ (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Rare-earth elements (REEs) are 17 elements of the periodic table primarily consisting of lanthanides. In modern society, the usage of REEs is ubiquitous in almost all modern gadgets and therefore efficient recovery and separation of REEs are of high importance. Selective adsorption and chelation of REEs in solid sorbents is a unique and sustainable process for their recovery. In this work, single-stranded oligos with 100 units of thymine were grafted onto carboxylated mesoporous carbon to synthesize a sorbent with phosphorus and oxygen functionalities. Additionally, the sorbent was characterized by X-ray photoelectron spectroscopy, Fourier-transform infrared spectroscopy, and scanning electron microscopy-energy-dispersive X-ray spectroscopy. Three different REEs with varying atomic radii and densities, Lu, Dy, and La, were adsorbed onto the carbon from aqueous solutions. It was observed that the adsorbed amounts increased with the increase in the atomic radius or decrease in the atomic density. Calculation of the distribution coefficients for all the equilibrium adsorption amounts suggested that adsorption is more effective in the lower concentration region. The L₃-edge X-ray absorption near-edge structure confirmed a 3+ oxidation state of REEs in the adsorbed phase. Extended X-ray absorption fine structure (EXAFS) confirmed the binding of REEs with oxygen functionalities in the adsorbed phase. The radial distribution functions calculated from the EXAFS data suggest a longer RE–O distance for La compared to those for Lu and Dy. The coordination numbers and Debye–Waller factors have typical values of about 8–9 atoms and 0.01–0.02 Å², respectively.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: European Research Council (ERC); National Science Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1842800

Report Number(s):: BNL-222657-2022-JAAM

Journal Information:: Langmuir, Journal Name: Langmuir Journal Issue: 1 Vol. 38; ISSN 0743-7463

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (36)

Hydration of Lanthanoid(III) Ions in Aqueous Solution and Crystalline Hydrates Studied by EXAFS Spectroscopy and Crystallography: The Myth of the “Gadolinium Break” Persson, Ingmar; D'Angelo, Paola; De Panfilis, Simone Chemistry - A European Journal, Vol. 14, Issue 10 https://doi.org/10.1002/chem.200701281	journal	March 2008
Determination of scandium, yttrium and lanthanides in silicate rocks and four new canadian iron-formation reference materials by flame atomic-absorption spectrometry with microsample injection Sen Gupta, J. Talanta, Vol. 31, Issue 12 https://doi.org/10.1016/0039-9140(84)80248-9	journal	December 1984
Fabrication, characterization, and biological assessment of multilayered DNA-coatings for biomaterial purposes van den Beucken, Jeroen J. J. P.; Vos, Matthijn R. J.; Thüne, Peter C. Biomaterials, Vol. 27, Issue 5 https://doi.org/10.1016/j.biomaterials.2005.06.015	journal	February 2006
Adsorption of rare earth elements onto bacterial cell walls and its implication for REE sorption onto natural microbial mats Takahashi, Yoshio; Châtellier, Xavier; Hattori, Keiko H. Chemical Geology, Vol. 219, Issue 1-4 https://doi.org/10.1016/j.chemgeo.2005.02.009	journal	June 2005
A simple approach to fabricate granular adsorbent for adsorption of rare elements Zhu, Yongfeng; Zheng, Yian; Wang, Aiqin International Journal of Biological Macromolecules, Vol. 72 https://doi.org/10.1016/j.ijbiomac.2014.08.039	journal	January 2015
Adsorptive recovery of neodymium and dysprosium in phosphorous functionalized nanoporous carbon Saha, Dipendu; Akkoyunlu, Sel Didem; Thorpe, Ryan Journal of Environmental Chemical Engineering, Vol. 5, Issue 5 https://doi.org/10.1016/j.jece.2017.09.009	journal	October 2017
A critical review on solvent extraction of rare earths from aqueous solutions Xie, Feng; Zhang, Ting An; Dreisinger, David Minerals Engineering, Vol. 56 https://doi.org/10.1016/j.mineng.2013.10.021	journal	February 2014
Adsorption of rare earth metals: A review of recent literature Anastopoulos, Ioannis; Bhatnagar, Amit; Lima, Eder C. Journal of Molecular Liquids, Vol. 221 https://doi.org/10.1016/j.molliq.2016.06.076	journal	September 2016
Extended X-ray absorption fine structure measurements of the local environment of Pr3+ ions in silica xerogels and zinc borate glasses Rocca, F.; Dalba, G.; Grisenti, R. Journal of Non-Crystalline Solids, Vol. 232-234 https://doi.org/10.1016/s0022-3093(98)00526-2	journal	July 1998
Studies on complexation and solvent extraction of lanthanides in the presence of diaza-18-crown-6-di-isopropionic acid Kim, J. Talanta, Vol. 45, Issue 2 https://doi.org/10.1016/s0039-9140(97)00151-3	journal	December 1997
Effect of pH on sorption for RE(III) and sorption behaviors of Sm(III) by D152 resin Xiong, Chunhua; Liu, Xiaozheng; Yao, Caiping Journal of Rare Earths, Vol. 26, Issue 6 https://doi.org/10.1016/s1002-0721(09)60020-x	journal	December 2008
Evaluation of D113 cation exchange resin for the removal of Eu(III) from aqueous solution Xiong, Chunhua; Zheng, Zhanwang Journal of Rare Earths, Vol. 28, Issue 6 https://doi.org/10.1016/s1002-0721(09)60231-3	journal	December 2010
Adsorption and desorption properties of D151 resin for Ce(III) Yao, Caiping Journal of Rare Earths, Vol. 28 https://doi.org/10.1016/s1002-0721(10)60324-9	journal	December 2010
Recovery of rare earth metals through biosorption: An overview Das, Nilanjana; Das, Devlina Journal of Rare Earths, Vol. 31, Issue 10 https://doi.org/10.1016/s1002-0721(13)60009-5	journal	October 2013
Adsorption of Rare Earth Elements onto DNA-Functionalized Mesoporous Carbon Unsworth, Colin E.; Kuo, Chin Chen; Kuzmin, Alexei ACS Applied Materials & Interfaces, Vol. 12, Issue 38 https://doi.org/10.1021/acsami.0c09393	journal	August 2020
Application of Freeze-Dried Powders of Genetically Engineered Microbial Strains as Adsorbents for Rare Earth Metal Ions Moriwaki, Hiroshi; Masuda, Reiko; Yamazaki, Yuki ACS Applied Materials & Interfaces, Vol. 8, Issue 40 https://doi.org/10.1021/acsami.6b08369	journal	September 2016
Noncompetitive and Competitive Adsorption of Heavy Metals in Sulfur-Functionalized Ordered Mesoporous Carbon Saha, Dipendu; Barakat, Soukaina; Van Bramer, Scott E. ACS Applied Materials & Interfaces, Vol. 8, Issue 49 https://doi.org/10.1021/acsami.6b12190	journal	November 2016
Highly Efficient and Selective Recovery of Rare Earth Elements Using Mesoporous Silica Functionalized by Preorganized Chelating Ligands Hu, Yimu; Drouin, Elisabeth; Larivière, Dominic ACS Applied Materials & Interfaces, Vol. 9, Issue 44 https://doi.org/10.1021/acsami.7b12589	journal	October 2017
Size-Selective Separation of Rare Earth Elements Using Functionalized Mesoporous Silica Materials Hu, Yimu; Misal Castro, Luis C.; Drouin, Elisabeth ACS Applied Materials & Interfaces, Vol. 11, Issue 26 https://doi.org/10.1021/acsami.9b04183	journal	May 2019
Covalent Modification of Multiwalled Carbon Nanotubes with Imidazolium-Based Ionic Liquids: Effect of Anions on Solubility Park, Min Jeong; Lee, Jae Kyun; Lee, Bang Sook Chemistry of Materials, Vol. 18, Issue 6 https://doi.org/10.1021/cm0511421	journal	February 2006
Evaluating Rare Earth Element Availability: A Case with Revolutionary Demand from Clean Technologies Alonso, Elisa; Sherman, Andrew M.; Wallington, Timothy J. Environmental Science & Technology, Vol. 46, Issue 6 https://doi.org/10.1021/es203518d	journal	February 2012
Adsorption of Neodymium(III) from Aqueous Solutions Using a Phosphorus Functionalized Adsorbent Park, Hyung-Jun; Tavlarides, Lawrence L. Industrial & Engineering Chemistry Research, Vol. 49, Issue 24 https://doi.org/10.1021/ie100403b	journal	December 2010
Strong and weak solvation steric effects on lanthanoid(III) ions in N,N-dimethylformamide–N,N-dimethylacetamide mixtures Ishiguro, Shin-ichi; Umebayashi, Yasuhiro; Kato, Kazusuke Journal of the Chemical Society, Faraday Transactions, Vol. 94, Issue 24 https://doi.org/10.1039/a806967k	journal	January 1998
Efficient adsorption and separation of dysprosium from NdFeB magnets in an acidic system by ion imprinted mesoporous silica sealed in a dialysis bag Zheng, Xudong; Liu, Enli; Zhang, Fusheng Green Chemistry, Vol. 18, Issue 18 https://doi.org/10.1039/c6gc01426g	journal	January 2016
Explicit local exchange-correlation potentials Hedin, L.; Lundqvist, B. I. Journal of Physics C: Solid State Physics, Vol. 4, Issue 14 https://doi.org/10.1088/0022-3719/4/14/022	journal	October 1971
Dehydration of the molybdenum trioxide hydrates MoO ₃ · n H ₂ O: in situ x-ray absorption spectroscopy study at the Mo K edge Kuzmin, Alexei; Purans, Juris Journal of Physics: Condensed Matter, Vol. 12, Issue 9 https://doi.org/10.1088/0953-8984/12/9/301	journal	February 2000
Extended x-ray-absorption fine-structure technique. III. Determination of physical parameters Stern, E. A.; Sayers, D. E.; Lytle, F. W. Physical Review B, Vol. 11, Issue 12 https://doi.org/10.1103/physrevb.11.4836	journal	June 1975
X-ray-absorption spectroscopy of a Nd 3 + -exchanged β’’-alumina crystal Rocca, F.; Kuzmin, A.; Purans, J. Physical Review B, Vol. 50, Issue 10 https://doi.org/10.1103/physrevb.50.6662	journal	September 1994
Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure Ankudinov, A. L.; Ravel, B.; Rehr, J. J. Physical Review B, Vol. 58, Issue 12 https://doi.org/10.1103/physrevb.58.7565	journal	September 1998
Extended x-ray absorption fine structure—its strengths and limitations as a structural tool Lee, P. A.; Citrin, P. H.; Eisenberger, P. Reviews of Modern Physics, Vol. 53, Issue 4 https://doi.org/10.1103/revmodphys.53.769	journal	October 1981
Theoretical approaches to x-ray absorption fine structure Rehr, J. J.; Albers, R. C. Reviews of Modern Physics, Vol. 72, Issue 3 https://doi.org/10.1103/revmodphys.72.621	journal	July 2000
Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides Shannon, R. D. Acta Crystallographica Section A, Vol. 32, Issue 5, p. 751-767 https://doi.org/10.1107/s0567739476001551	journal	September 1976
EXAFS study of Tb-doped silica xerogels Rocca, F.; Monti, F.; Kuzmin, A. Journal of Synchrotron Radiation, Vol. 6, Issue 3 https://doi.org/10.1107/s0909049598016252	journal	May 1999
Recovery and Separation of Rare Earth Elements Using Salmon Milt Takahashi, Yoshio; Kondo, Kazuhiro; Miyaji, Asami PLoS ONE, Vol. 9, Issue 12 https://doi.org/10.1371/journal.pone.0114858	journal	December 2014
Recovery and Separation of Rare Earth Elements Using Columns Loaded with DNA-filter Hybrid Takahashi, Yoshio; Kondo, Kazuhiro; Miyaji, Asami Analytical Sciences, Vol. 28, Issue 10 https://doi.org/10.2116/analsci.28.985	journal	January 2012
Soft-Templating of Sulfur and Iron Dual-Doped Mesoporous Carbons: Lead Adsorption in Mixtures Saha, Dipendu; Richards, Connelly P.; Haines, Robert G. Molecules, Vol. 25, Issue 2 https://doi.org/10.3390/molecules25020403	journal	January 2020

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